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Reactivity of the O2+·(H2O)n and NO+·(H2O)n cluster ions in the D-region of the ionosphere†
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2018-10-02 00:00:00 , DOI: 10.1039/c8cp05681a Sainish Sharma 1, 2, 3 , Timothy G. Wright 1, 2, 3 , Nicholas A. Besley 1, 2, 3
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2018-10-02 00:00:00 , DOI: 10.1039/c8cp05681a Sainish Sharma 1, 2, 3 , Timothy G. Wright 1, 2, 3 , Nicholas A. Besley 1, 2, 3
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The protonated water clusters present in the D-region of the ionosphere have been postulated to be formed from cluster ions such as O2+·(H2O)n and NO+·(H2O)n, although the detailed mechanism of the underlying reactions is not understood. Second order Møller–Plesset perturbation theory based Born–Oppenheimer ab initio molecular dynamics (AIMD) simulations of the reactions of the O2+·(H2O)n and NO+·(H2O)n cluster ions to form protonated water clusters reveal different mechanisms for the O2+ and NO+ based ions. AIMD simulations of O2+·(H2O)n=2–5 with initial velocities of the atoms sampled from the Maxwell–Boltzmann distribution at 220 K show that following charge transfer, a reaction to form a protonated water cluster and OH occurs rapidly where the neutral O2 molecule is just a spectator. In contrast, the reaction of NO+·(H2O)n=4,5 has been hypothesised to involve an intracluster reaction, but no reaction is observed in AIMD simulations using thermal initial velocities. However, it is shown that reactions to form protonated water clusters do occur in simulations when a water molecule collides with a NO+·(H2O)4 cluster.
中文翻译：
电离层D区域中 O 2 + ·（H 2 O）n和NO + ·（H 2 O）n簇离子的反应性†
据推测，存在于电离层D区的质子化水团簇是由团簇离子形成的，例如O 2 + ·（H 2 O）n和NO + ·（H 2 O）n。根本的反应还不清楚。基于二阶Møller-Plesset微扰理论的O 2 + ·（H 2 O）n与NO + ·（H 2 O）n反应的Born-Oppenheimer从头算分子动力学（AIMD）模拟形成质子化水团簇的离子揭示了基于O 2 +和NO +的离子的不同机理。AIMD对O 2 + ·（H 2 O）n = 2–5的模拟，从麦克斯韦-玻耳兹曼分布在220 K处采样的原子的初始速度表明，电荷转移后，发生了形成质子化水团和OH的反应中性O 2分子只是一个旁观者。相反，NO + ·（H 2 O）n = 4,5的反应假设已经涉及到团簇内反应，但是在使用热初始速度的AIMD模拟中未观察到任何反应。然而，表明在模拟中当水分子与NO + ·（H 2 O）4团簇碰撞时，确实发生了形成质子化水团簇的反应。
更新日期：2018-10-02
中文翻译：
电离层D区域中 O 2 + ·（H 2 O）n和NO + ·（H 2 O）n簇离子的反应性†
据推测，存在于电离层D区的质子化水团簇是由团簇离子形成的，例如O 2 + ·（H 2 O）n和NO + ·（H 2 O）n。根本的反应还不清楚。基于二阶Møller-Plesset微扰理论的O 2 + ·（H 2 O）n与NO + ·（H 2 O）n反应的Born-Oppenheimer从头算分子动力学（AIMD）模拟形成质子化水团簇的离子揭示了基于O 2 +和NO +的离子的不同机理。AIMD对O 2 + ·（H 2 O）n = 2–5的模拟，从麦克斯韦-玻耳兹曼分布在220 K处采样的原子的初始速度表明，电荷转移后，发生了形成质子化水团和OH的反应中性O 2分子只是一个旁观者。相反，NO + ·（H 2 O）n = 4,5的反应假设已经涉及到团簇内反应，但是在使用热初始速度的AIMD模拟中未观察到任何反应。然而，表明在模拟中当水分子与NO + ·（H 2 O）4团簇碰撞时，确实发生了形成质子化水团簇的反应。
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